Evolution of microstructural damage in coal under supercritical CO₂-water exposure: A multi-scale study incorporating the indentation size effect

Authors

  • Bozhi Deng State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400030, P. R. China
  • Bingyang Jiao State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400030, P. R. China
  • Baisheng Nie* State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400030, P. R. China (Email: bshnie@cqu.edu.cn)
  • Changbao Jiang* State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400030, P. R. China (Email: JCB@cqu.edu.cn)
  • Minghui Li State Key Laboratory of Intelligent Construction and Healthy Operation and Maintenance of Deep Underground Engineering, Shenzhen University, Shenzhen 518060, P. R. China; Guangdong Provincial Key Laboratory of Deep Earth Sciences and Geothermal Energy Exploitation and Utilization, Shenzhen University, Shenzhen 518060, P. R. China
  • Yumeng Zhao Department of Civil and Environmental Engineering, University of Nebraska-Lincoln, Omaha 68106, USA

Abstract

CO₂ sequestration in coal seams represents an effective strategy for mitigating CO₂ emissions. However, the complicated interaction of CO₂-water-coal at the micro-scale may compromise the structural integrity and mechanical strength of coal, thereby adversely impacting the efficacy and safety of CO₂ sequestration in coal seams. This study introduces a novel indentation testing method that reveals the scale-dependent evolution mechanisms of coal microstructures, enabling the accurate and reliable quantification level of degradation in the micromechanical properties caused by supercritical CO₂ water-coal interactions. Using this method, the extent of mechanical degradation in three types of coal microstructures could be accurately evaluated under supercritical CO₂ water-coal interaction. The pure organic matrix exhibited remarkable stability under all fluid treatments, with minor changes in microstructure feature and a mechanical property reduction of less than 25%. In contrast, the mineral structures were significantly altered by treatment with fluid mixed with supercritical CO₂ and brine, with erosion depths and mechanical property reductions reaching 1.6 µm and 80% in granular structures, and 6.4 µm and 90% in banded structures. However, in the absence of brine or supercritical CO₂, the erosion depths and mechanical property reductions of fusinite were limited.

Document Type: Original article

Cited as: Deng, B., Jiao, B., Nie, B., Jiang, C., Li, M., Zhao, Y. Evolution of microstructural damage in coal under supercritical CO₂-water exposure: A multi-scale study incorporating the indentation size effect. Advances in Geo-Energy Research, 2025, 17(3): 212-225. https://doi.org/10.46690/ager.2025.09.04

Keywords:

CO₂-water-coal interaction, nanoindentation, erosion quantification, indentation size effect, micromechanical properties

References

Armitage, P. J., Faulkner, D. R., Worden, R. H. Caprock corrosion. Nature Geoscience, 2013, 6(2):79-80.

Bashir, A., Ali, M., Patil, S., et al. Comprehensive review of CO2 geological storage: Exploring principles, mechanisms, and prospects. Earth-Science Reviews, 2024, 249: 104672.

Chen, B., Harp, D. R., Zhang, Y., et al. Dynamic risk assessment for geologic CO2 sequestration. Gondwana Research, 2023, 122: 232-242.

Chen, K., Liu, X., Nie, B., et al. Mineral dissolution and pore alteration of coal induced by interactions with supercritical CO2. Energy, 2022, 248: 123627.

Chua, J., Zhang, R., Chaudhari, A., et al. High-temperature nanoindentation size effect in fluorite material. International Journal of Mechanical Sciences, 2019, 159: 459-466.

Deng, B., Nie, B., Liu, X., et al. Characteristics of the heterogeneous mechanical response of coal at the nano and micro-scale using instrumented indentation experiments. Chinese Journal of Theoretical and Applied Mechanics, 2022, 54(8): 2304-2317. (in Chinese)

Ebisu, T., Horibe, S. Analysis of the indentation size effect in brittle materials from nanoindentation load-displacement curve. Journal of the European Ceramic Society, 2010, 30(12): 2419-2426.

Fender, T. D., Rouainia, M., Van Der Land, C., et al. Geomechanical properties of coal macerals; measurements applicable to modelling swelling of coal seams during CO2 sequestration. International Journal of Coal Geology, 2020, 228: 103528.

Friedlingstein, P., O’Sullivan, M., Jones, M. W., et al. Global carbon budget 2024. Earth System Science Data, 2025, 17(3): 965-1039.

Gathitu, B. B., Chen, W., McClure, M. Effects of coal interaction with supercritical CO2: Physical structure. Industrial &Engineering Chemistry Research, 2009, 48(10): 5024-5034.

Han, Q., Chen, P., Ma, T. Influencing factor analysis of shale micro-indentation measurement. Journal of Natural Gas Science and Engineering, 2015, 27: 641-650.

He, H., Liu, P., Nie, B., et al. Micromechanical property evolution and damage mechanism of coal subjected to ScCO2 treatment. Energy, 2024, 304: 132087.

Jiang, C., Xu, W., Deng, B., et al. Mineral erosion in different microstructures under ScCO2-water-coal interactions: Implications for CO2 sequestration in coalbeds. Energy & Fuels, 2025, 39(9): 4374-4394.

Jiang, R., Yu, H. Interaction between sequestered supercritical CO2 and minerals in deep coal seams. International Journal of Coal Geology, 2019, 202: 1-13.

Joslin, D. L., Oliver, W. C. A new method for analyzing data from continuous depth-sensing microindentation tests. Journal of Materials Research, 1990, 5(1): 123-126.

Kossovich, E. L., Borodich, F. M., Epshtein, S. A., et al. Indentation of bituminous coals: Fracture, crushing and dust formation. Mechanics of Materials, 2020, 150: 103570.

Kossovich, E., Epshtein, S., Krasilova, V., et al. Effects of coals microscale structural features on their mechanical properties, propensity to crushing and fine dust forma tion. International Journal of Coal Science & Technology, 2023, 10(1): 20.

Li, M., Chen, W. Factors resulting in micron indentation hardness descending in indentation tests. Chinese Journal of Aeronautics, 2009, 22(1): 43-48.

Liu, T., Li, M., Li, J., et al. Interactions of CO2-H2O coal and its impact on micro mechanical strength of coal. Geoenergy Science and Engineering, 2023a, 227: 211915.

Liu, A., Liu, S. Mechanical property alterations across coal matrix due to water-CO2 treatments: A micro-to-nano scale experimental study. Energy, 2022, 248: 123575.

Liu, S., Sang, S., Ma, J., et al. Effects of supercritical CO2 on micropores in bituminous and anthracite coal. Fuel, 2019, 242: 96-108.

Liu, B., Yao, J., Sun, T. Numerical analysis of water alternating-CO2 flooding for CO2-EOR and storage projects in residual oil zones. International Journal of Coal Science & Technology, 2023b, 10(1): 73.

Luo, S., Lu, Y., Wu, Y., et al. Cross-scale characterization of the elasticity of shales: Statistical nanoindentation and data analytics. Journal of the Mechanics and Physics of Solids, 2020, 140: 103945.

Manika, I., Maniks, J. Size effects in micro- and nanoscale indentation. Acta Materialia, 2006, 54: 2049-2056.

Manjunath, G. L., Akono, A. T., Haljasmaa, I., et al. Role of CO2 in geomechanical alteration of morrow sandstone across micro-meso scales. International Journal of Rock Mechanics and Mining Sciences, 2023, 163: 105311.

Masoudian, M. S., Airey, D. W., El-Zein, A. Experimental investigations on the effect of CO2 on mechanics of coal. International Journal of Coal Geology, 2014, 128-129: 12-23.

Meng, M., Qiu, Z. Experiment study of mechanical properties and microstructures of bituminous coals influenced by supercritical carbon dioxide. Fuel, 2018, 219: 223-238.

Mouallem, J., Al-Abdrabalnabi, R., Raza, A., et al. Experi mental investigation of CO2 residual trapping in naturally water-wet and artificially tailored oil-wet limestones: Implications for geological CO2 storage. Advances in Geo-Energy Research, 2025, 17(1): 43-55.

Mukhopadhyay, N. K., Paufler, P. Micro- and nanoindentation techniques for mechanical characterisation of materials. International Materials Reviews, 2006, 51(4): 209-245.

Nie, B., He, H., Liu, P., et al. Nanomechanical behavior of coal with heterogeneous minerals and pores using nanoindentation. Environmental Science and Pollution Research, 2024, 31(19): 28007-28024.

Niu, Q., Wang, X., Chang, J., et al. Influencing mechanisms of multi-scale pore-fracture responses of coals on their macro/micromechanical behaviors under ScCO2 injection. Advances in Geo-Energy Research, 2024, 14(1): 64-80.

Perera, M. S. A., Ranjith, P. G., Viete, D. R. Effects of gaseous and super-critical carbon dioxide saturation on the mechanical properties of bituminous coal from the Southern Sydney Basin. Applied Energy, 2013, 110: 73-81.

Safaei-Farouji, M., Misch, D., Sachsenhofer, R. F., et al. CO2 utilization and sequestration potential in deep coal seams: A case study on carboniferous coals from the Karaganda basin, kazakhstan. Journal of CO2 Utilization, 2025, 101: 103204.

Sampath, K. H. S. M., Perera, M. S. A., Ranjith, P. G., et al. CO2 interaction induced mechanical characteristics alterations in coal: A review. International Journal of Coal Geology, 2019, 204: 113-129.

Shen, W., Ma, T., Zuo, L., et al. Advances and prospects of supercritical CO2 for shale gas extraction and geological sequestration in gas shale reservoirs. Energy & Fuels, 2024, 38(2): 789-805.

Shi, F., Deng, B., Nie, B., et al. Deformation kinetics of coal-gas system during isothermal and dynamic non isothermal processes. Gas Science and Engineering, 2023, 117: 205027.

Siqueira, T. A., Iglesias, R. S., Ketzer, J. M. Carbon dioxide injection in carbonate reservoirs– a review of CO2-water rock interaction studies. Greenhouse Gases: Science and Technology, 2017, 7(5): 802-816.

Su, E., Liang, Y., Chen, X., et al. Relationship between pore structure and mechanical properties of bituminous coal under sub-critical and super-critical CO2 treatment. Energy, 2023, 280: 128155.

Sundal, A., Hellevang, H. Using reservoir geology and petrographic observations to improve CO2 mineralization estimates: Examples from the Johansen formation, North Sea, Norway. Minerals, 2019, 9(11): 671.

Wang, P., Gao, Y., Wang, P. A comparative study of indentation size effect models for different materials. Scientific Reports, 2024, 14(1): 20010.

Wang, J., Yang, C., Liu, Y., et al. Using nanoindentation to characterize the mechanical and creep properties of shale: Load and loading strain rate effects. ACS Omega, 2022, 7(16): 14317-14331.

Wu, Q., Zhu, C. Enhancement of carbon sequestration capacity of coal through long-term geochemical reactions with ScCO2-H2O. Energy & Fuels, 2025, 39(32): 15400 15417.

Xu, S., Zhou, S., Zhou, J., et al. Multiscale pore structure evolution of Longmaxi shale induced by acid treatment. SPE Journal, 2022, 28(2): 831-844.

Yang, C., Xiong, Y., Wang, J., et al. Mechanical characterization of shale matrix minerals using phase-positioned nanoindentation and nano-dynamic mechanical analysis. International Journal of Coal Geology, 2020, 229: 103571.

Zagorščak, R., Thomas, H. R. Effects of subcritical and supercritical CO2 sorption on deformation and failure of high-rank coals. International Journal of Coal Geology, 2018, 199: 113-123.

Zhang, L., Chen, L., Hu, R., et al. Subsurface multiphase reactive flow in geologic CO2 storage: Key impact fac tors and characterization approaches. Advances in Geo Energy Research, 2022a, 6(3): 179-180.

Zhang, F., Guo, H., Hu, D., et al. Characterization of the mechanical properties of a claystone by nano-indentation and homogenization. Acta Geotechnica, 2018, 13(6): 1395-1404.

Zhang, G., Ranjith, P. G., Lyu, Q. Direct evidence of CO2 softening effects on coal using nanoindentation. Energy, 2022b, 254: 124221.

Zhang, C., Wang, Y., Kou, Z., et al. Recent research advances in enhanced CO2 mineralization and geologic CO2 storage. Advances in Geo-Energy Research, 2023, 10(3): 141-145.

Zhou, Z., Sheng, M., Ge, Z., et al. Mechanical properties and failure characteristics of supercritical carbon dioxide soak in water-bearing coal rocks. Energy, 2024, 286: 129599.

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Published

2025-08-27